Fractional fusion apparatus



Odie ZI, 1952 j, G, A51-QN 5TMb *25614,909

FRACTIONAL FUSION APPARATUS vFiled Feb. 21, 1950 ..2SHEETs-SHEET 1 PTV.

JNVENTORS.

J. GL ASTON S.V.R.MASTRANGELO ATTORNEYS Olct. 2l, 1952 J. G. AS'TN ETAL 2,614,909

' FRACTIONAL FUSION APPARATUS Filed Feb. 21. 195o. 2 sr-.xEETs--SHEET 2 IN V EN TORS. J.'G'. ASTON BY S .V. R. MASTRANGELO A T TURNE YS Patented Oct. 21, 1952 NUNITED r STATES PATENT olflrl'czrz-l John G. Aston and Sebastiani `V.R'. Mastrangelo;

State College;` Pa., assignors to .Phillips Petrloleum Company, a corporation of Delaware Applicaiionrebruaryzi, 1950,;scria`l No. 145,404. d

` Claims. (C1. 23-280) This Vinvention Arelates lto the purification of impure materials. AIn one aspect, itrelates to apparatus for removing impurities from an impure material. In another aspect;l it relates to apparatus for puriiication by fractional fusion. In still another aspect, it relates 4toapparatus for accelerating the adiabatic attainment of state equilibrium in a mass of granular material in contact with a liquid of the'same components.

In the purication of compounds 'or the sepa-` ration of mixtures of compounds by fractional fusion, `one of `the diiculties arises from the fact that state equilibriumcannot be rapidly attained. This is partly due to the fact that the solid and liquid do not move about Within the system and heat transfer between the phases is v slow. If the material tobe purified has a very low freezing point, the use of mechanical agita tion presents so many diiculties that it is used onlyi as a last resort.

We have discovered an apparatus wherein the,

adiabatic attainment of state `equilibrium is `considerably accelerated without using` mechanical agitation.` Our invention is particularlyuseful in the purification of low-melting compounds by the fractional fusion method. In our apparatus,`

we provide a closed, thermally insulatedsample or material receiving container with meansfor controlling the rate and amount of heat added to the material to be p uried. Inside the thermally insulated containenwe provide aheat conducting material. Heat added to the container at one pointis rapidly transferred to all parts of the material within the container.

vThe principal object cf our invention is to provide an apparatus 'for lowftemperature fractional fusion separations.

Another object is to `provide a means for lac celerating the adiabatic attainment of state equilibrium within the `body of a samplebeing purified.

`Anotherobject is to provide an apparatus lfor ratus `wherein the "heat-dispersing means is a spiral lmetal `ribbon Vwitlfi means for compressing the spiral ribbon to squeeze out-any liquid contained in thesolid trapped between "the van-es. Figure 4 is anothermodilcation of our appa.-

ratus whereiny the heat-dispersing means is a plurality of horizontal `metal plates which are tted onto "vertical guide rods fand jvvhich `are held apart by means of spiralfsprings which ride onthe guide rods betweensaid platesi. I

In Figure 1,\an outer closedV container 6 is provided With an Yevacuation tube l. Inside the outer container is aclosely-tting *closed container B vof a heatradiating material. Inside container 8 is a smaller, closed container '9, around the periphery of which area number of turns of Wire II `for heating container 9.- -.Between.radia tion` shield f8 and container 9 is alayerof insulating `material I2, 'such as cork. Inside con-I tainer1 `9 is another layer `of insulating material I3, insideof which is `a sample container IIl comprising a closed vessel around the outerperiphery` oi?` which is Wound an electrical theater I6. Inside container I4 is a .vertically-positionedloosely-wound roll .of wire gauze Il. A filling tube I8 extendsffrom the outsidezof container 6 rapidly transferring heatthroughout a sample" rial `in the container is a loosely-wound roll of the I following Figure 2 is a cross sectional View ofthe apparatus Vshown in Figure 1 taken along line22.

`Figure is anothermodication of our appatothe top of inner container III. `'Ihevelectrical leads forthe heaters I land I6 pass from the out-f. side to the inside of the apparatus throughcon` duit;` I9. A'liquid-removal tube-2I leads from the bottom of the sample container through the top to the outside. Inside tube 2l is a conduction heater 22. In `this case, the `conduction heater is a Wire which is electricallytheated. At the bottom of tube 2| is a drilledplug 23 above which. is a porous plug 24. 1

In Figure 2, the spiral gauze I'I ismore clearly shown vwith relation to inner container |4151 In Figure :3, radiation shield 26 ts closely inside outer container 21. A pumping tube .30` isA provided forfevacuating the system. Supported within. the radiation shield 23 `by means lof "a layer of4 insulating. material `28 'is'aheater shield 29 which is heated by means of an` electrical heater 3| `Wound around the outside.l .spaced within the heater shield 29 by means of allayer of insulation'32 is a vsample container 33. Extending upwardly into `said Vsample container is a heater Well 3Iland` heater 36. Inside container 33 is a spiral ribbon 31,` the bottom turn of which is secured to the bottom of container "33;and the top turn of which is Vsecured to an vactivator vane l 38which1its slidablyover the top of heater `wellh 34 and which 'also liits slidably ,into `colurrniQ39 which extends upwardly from heater shield 29.'

At the upper extremity of tube 39 is a sealing gland 4! through which activator rod 42 extends downwardly to activator vane 38 to which it is secured. At a point intermediate the extremities of the tube 39, a side tube 43 enters said tube 39 for introducing material into sample container 33. Openings 44 in the top of activator vane 38 permit liquid introducedthroughtube 43 toiiow into container 33.

A thermocouple 46 is provided for controlling the heat added through heater shield 29 according to the temperature difference between .the inner wall of heater shield 29 and the outer wall of sample container 33 as heatery35 and thermo-f` couple 36 extend upwardlyinto heater well 34 for heating container 33. The electrical leads for heater 35, thermocouple 36, heater 3l, and

' such as copper, and contain numerous perforations to permit flow of liquid therethrough. The

material to be processed is introduced into the containerby means of side tube 43 and tube 38. 'The freezing and melting process is carried out as'described above.

The liquid is drawn oi Y .through removal tube 48 after pressure has been thermocouple 4B enter the apparatus through e' conduit 41.

A product removal tube 48 extends from the outside to the bottom' of container 33, and runningy along the lengthof` said tube inside is a conduction heater 49, At the bottom of tube 48 is a drilledzplug 5lk and` a porous plug 52 which filter solids out of the liquid being removed.

The apparatus shownin Figure 4 is a modification of-.jthat shown in Figure 1 wherein the roll of gauze is replaced by a series `of horizontal plates 56` which ride on vertical guides 5l and are held apart by means of spiralsprings 58 whichit on said vertical guides. An activating rod 5S kextends upward from the uppermost horizontal Thead'vantagesof vouryinvention will be more clearlyI understood from the following description ofthe method of operation. The apparatus shown in Figure 1 consists of an inner container, preferably copper,which is provided with a heater'vl and thermocouple l5. 'A roll of wire gauze fl'is placed in the container. This gauze may be' of any conducting material which does not react with the material being processed. We have found copper to be an excellent material for this purpose. This wire gauze serves to facilitate equilibrium by rapidly equalizing the temperature throughout the sample. t also tends to expose a larger crystal surf-ace to the equilibrium liquid since the crystals tend to form on the gauze surface.- f-

The material to be processed is introduced into the material receiving container I4 through lling tube i 8. The material may be introduced as a granular solid, as a slurry, or as a liquid, preferably `the latter. If lthe material is introduced as a liquid, it mustthen-be frozen inside the container by passing a cold gas through the liquid by means of the withdrawal tube 2l, or by surrounding the outer container 6 with avrefrigeratl ing liquid; After the liquid within the container has been frozen, sufiicient heat is added to melt that` portion which. will contain the impurity. Then,y by suitably adjusting the heat input to the thermal shield S, there isno heat interchange between the container and its surroundings. After attaining equilibrium'adiabatically the liquid is Awithdrawn through removal tube 2 l The heat is againadded to the system by means of heater l@ to meltr an additional portion of the solid within.th.e'container.. .After the fiow of heat into the container has been stopped, the liquid and the remaining solidl are once again allowed to equilibrate 'adiabatically. The liquid is then with'-` Y pure state.

' applied to the vanes by means of activating rod 42 and activator vane 38. The solid material is pressed between the spiral vanes, which aids in removal of liquid Afrom the solid. During. the equilibrating period when the solid and liquid are in contact, the activator vane may be recip- 53 have numerous periorations topermit ow of liquid from one section of ,the adjoining ones.

Springs .58, which work on the guide rods 5l tend, Plates 56.

to keep these plates forced apart. are constructed of a heat conducting material so that heat added to one portion of the sample willv be rapidly transmitted throughout the sample. Activator rod 59 is used to force the piates 56 together and express `the liquid from the solid. This activator rod and metal piates may be used also to provide a certain amount of agitation within the sample during the equilibrating period.

Our apparatus may be used in the separation of eutectic-forming mixtures as well as solid solution-forming mixtures. f'the sample to be processed is a eutectic-forming mixture, substantial;`

ly all of the impurity can be removed by a single melting. Additional meltings may be desirable',l

to remove any occluded liquid. If. the impurity is solid-soluble with a distribution favoring theV liquid phase, a plurality of meltings is desirable.` The exact amount of the sample to ,-be melted each time and the number of meltings to be emv ployed depends on the individualsampleland may be easily determined.

Our invention is applicable to any system wherein the components are not decomposed by Obviously, the apparatus of this type -is more useful in the separation of extremely melting.

low-melting materials which are valuable in the Examples are the separation of,v cis and trans-butene-2, meta and-para xylenes, normal hexane andbenzene, and other materialsA which melt below atmospheric g temperatures,

However, our invention is not limited to these only by the following claims. f

Having described our invention, we claim:I l 1. Afractional fusionapparatus which-'coup prises in combination, a closed material receiving container; an upright mass of heat-conducting gauze within and extending throughout the length of said material receiving container; at least one rst electrical heating element closely contacting the periphery of said material receiving container; a rst layer of insulation material covering the surface of said material receiving container and said rst heating element; a closed heater shield chamber closely fitted around said iirst layer of insulation; at least one second electrical heating element closely contacting the periphery of said heater shield chamber; a second layer of insulation covering the surface of said heater shield chamber and said second electrical heating element; a closed radiation shield chamber closely iitted around said second layer of insulation; a closed outer container closely iitted around the periphery oi said radiation shield chamber; a lling tube extending from outside said outer container into said material receiving container; a liquid product removal conduit extending from the lower portion of said container to the exterior of said apparatus; .and means to evacuate said outer container.

2. A fractional fusion apparatus which comprises in combination, a closed material receiving container; heat distribution means within said material receiving container comprising a loosely-wound spiral perforate ribbon substantially iilling said container and having an opening therethrough; a heater well extending from the bottom of said material receiving container upwardly through the opening in said ribbon, forming a guide therefor; at least one first electrical heating element closely contacting the periphery of said material receiving container; a iirst layer of insulation material covering the surface of said material receiving container and said first heating element; a closed heater shield chamber "i closely fitted around said iirst layer of insulation; at least one second electrical heating element closely contacting the periphery of said heater shield chamber; a second layer of insulation covering the surface of said heater shield chamber and said second electrical heating element; a closed radiation shield chamber closely fitted around said second layer of insulation; a closed outer container closely fitted around the periphery of said radiation shield chamber; means for compressing and decompressing said spiral ribbon extending from outside said outer container into said material receiving container and operatively connected to said spiral ribbon; a iilling tubev extending from outside said outer container into said material receiving container; a liquid product removal line extending from the lower portion of said container to the exterior of said apparatus; and means to evacuate said outer container.

3. A fractional fusion apparatus which comprises in combination, a closed material receiving container; heat distribution means Within said material receiving container comprising a plurality of plates slidably and horizontally disposed throughout said material receiving `container and supported on vertical guide rods; springs on said guide rods, adapted so as to non-rigidly space said plates apart; at least one first electrical heating element closely contacting the periphery of said material receiving container;

a. first layer of insulation material covering the surface of said material receiving container and said first heating element; a closed heater shield chamber closely fitted around said rst layer of insulation; at least one second electrical heating element closely contacting the periphery of said heater shield chamber; a second layer of insulation covering the surface of said heater shield chamber and said second electrical heating element; a closed radiation shield chamber closely fitted around said second layer of insulation; a closed outer container closely fitted around the periphery of said radiation shield chamber; means for moving said plates together and apart, extending from outside said buter` container into said material receiving container and operatively connected to said plates; a lilling tube extending from outside said outer container into said material receiving container; a liquid product removal line extending from the lower portion of said container to the exterior of said apparatus; and means to evacuate said outer' container.

4. A fractional fusion apparatus which comprises in combination, a closed material receiving container; heat distribution means within said material receiving container and extending throughout that container; at least one first electrical heating element closely contacting the periphery of said material receiving container; a first layer of insulation material covering the surface of said material receiving container and said rst heating element; a closed heater shield chamber closely fitted around said iirst layer of insulation; at least one second electrical heating element closely contacting the periphery oi said heater shield chamber; a second layer of insulation covering the surface of said heater shield chamber and said second electrical heating element; a closed radiation shield chamber closely fitted around said second layer of insulation; a closed outer container closely fitted around the periphery of said radiation shield chamber; a filling tube extending from outside said outer container into said material receiving container; a liquid product removal line extending from the lower portion of said container to the exterior of said apparatus; and means to evacuate said outer container.

5. The fractional fusion apparatus of claim 4. wherein a porous plug is provided in the inlet end of said liquid product removal line.

JOHN G. ASTON. SEBASTIAN V. R. MASTRANGELO.

REFERENCES CITED The following references are of record in the le of this patent:

UNiTED s'rA'rEs PATENTS Number Name Date 1,929,511 Mulkey Oct. 10, 1933 1,943,749 Trent Jan. 16, 1934 1,967,185 Clapp July 17, 1934 2,112,743 Poole Mar. 29, 1938 2,499,043 Voorhees Feb. 28 1950 FOREIGN PATENTS Number Country v Date 441,283 Germany Mar. 1, 1927 

1. A FRACTIONAL FUSION APPARATUS WHICH COMPRISES IN COMBINATION, A CLOSED MATERIAL RECEIVING CONTAINER; AN UPRIGHT MASS OF HEAT-CONDUCTING GAUZE WITHIN AND EXTENDING THROUGHOUT THE LENGTH OF SAID MATERIAL RECEIVING CONTAINER; AT LEAST ONE FIRST ELECTRICAL HEATING ELEMENT CLOSELY CONTACTING THE PERIPHERY OF SAID MATERIAL RECEIVING CONTAINER; A FIRST LAYER OF INSULATION MATERIAL COVERING THE SURFACE OF SAID MATERIAL RECEIVING CONTAINER AND SAID FIRST HEATING ELEMENT; A CLOSED HEATER SHIELD CHAMBER CLOSELY FITTED AROUND SAID FIRST LAYER OF INSULATION; AT LEAST ONE SECOND ELECTRICAL HEATING ELEMENT CLOSELY CONTACTING THE PERIPHERY OF SAID HEATER SHIELD CHAMBER; A SECOND LAYER OF INSULATION COVERING THE SURFACE OF SAID HEATER SHIELD CHAMBER AND SAID SECOND ELECTRICAL HEATING ELEMENT; A CLOSED RADIATION SHIELD CHAMBER CLOSELY FITTED AROUND SAID SECOND LAYER OF INSULATION; A CLOSED OUTER CONTAINER CLOSELY FITTED 